Composition for ceramic uses, and method of making the same



' later stated, I have Patented Nov. 10, 1931 umrsn ST'ATESPATENT osmosmzoius a. mm, or moron rum, nos momma. cams-0min, ABSIGNOB, BY

1mm ASSIGNMENTS, T0 PACIFIC-SOUTHWEST TRUST &- SAVING-B BANK, TRUSTEE,

or no; mamas, cnnoama, a coarons'rrox or car-moans oonosrrrox a cminc usm, urn IE'IIIOD or name m sum Io Drawing.

In the develo ment of the ceramic arts there have been iscoveredifromtimeto time certain mineral substances that when added to ceramic materials, will enhance greatly I the strength thereof, and possibly afford other-advantageous qualities, in the products made from such materials. Such products may'embrace for instance, all, objects made from burnt cit Minerals of the Stillmanits class have een found quite valuable in improving ceramic products by groducmg superior strength therein. Butsuc minerals are relatively scarce, and where found,-are located in laces of inaccessibility such that the cost 0? mining and bringing them to places of lproduction makes them quite er:- pensive.' or many applications, or ceramic uses, which. I have 'in' mind therefore thls cost of sillimanite makes its employment prohibitive. a

Desirous of using some mineral substance for the purposes su ges'ted, and'others to be iad recourse to the mineral known as pyrophyllite ore which is composed of hydrous aluminum.silicate. This is found in relatively large quantities in several sections of this country, 'andwhile in its crude state associated with various products of decomposition (not now known) and metamor hism, it is not available for mfy purposes, have devised a special mode 0 treatment of the same whereby I produce a composition having substantiall all the properties of the sillimanite class 0 minerals 35 as used for ceramic purposes. Owin to a the availability of pyrophyllite ore in arge quantities close to production points, my composition made t erefrom may be products, by way, of resistance to impact is anced. Moreover, by add tremendously en pro-' duced at much less cost than any for. the,

Application ma leptember a, Serial No. mar.

ing my composition to the clay, the'absence of addltion of fluxes, I have. found an important increase in toughness, which in other words, may be expressed as tensile,

cross-breaking, and compressive strength, while not producing hardness. The foregoing are 0 vious desiderata in the art.

Tests show that where hardness is required, the same may be achieved'by su plymg an admlxture of my composition, an clay, with any of the customary fluxes such as magnesium carbonate, etc. There is thus provided a porcelain-like mass havin a hardcreased porosity in the final fired product.

The degree of porosity is largely in lirect proportion to the amount of the composition added. This base of action of my invention is highly important for it may promote the'insulating qualities of certain ultimate burned clay products such as terra cotta building material, bricks, hollow tile, etc.

In practical terms,.the composition of my. invention 'is found to possess another im portant characteristic. Added to clay 1t neutralizes or reduces the firing shrinkage of the clay doubtless due to its own ex ansion. Thus where fired clay objects must made a'ccuratel to size, complete results will be attained y ro erly proportioning my composition an c ay mixture so that neither expansion, nor shrinkage, of the molded article will be obtained.

From the view point of refracto properties my composition discloses an er test that when mixed with ball clay or fire clay the melting point is increased. almost in the proportions of the percentage of "composition added. Admixed alone as a cement or grout, with plastic fire clay, my composition is of sin ular value in eliminating fire shrinkage of c ay bodies.

In the carrying out of myinvention; the

. tain impurities that areremoved therefrom by my process of treatment. These impurities largely are iron oxide, titanium oxide, lime and magnesia. Were the metallic oxides not removed they would produce discoloration andspecks 1n the final product. The lime and magnesia are undesirable owing to their fluxin influence when the prod not to be made is ar refractory purposes.

By careful microscopic examination on various sized gra' s produced by crushing rolls and other milling machinery, it has been determined that most ofthe lime and magnesia of pyro hyllite ore occur in a claylike substance w ich apparently had been de osited in the seams of the ore by water in ltration from above. The iron oxide and titania are found to be present chiefly in a cigstalline mineral believed to be tourmaline w ich is found scattered throughout the ore in small particles. A certain amount of free quartz occurs in the veins but most of this can readily be removed by rough hand sortin ily process for Purification of the ore or pyrophyllite is as ollows:

The crude ore in lumps a groximately five inches diameter, is charge into a special type of furnace known as the Curtis converter. The operation in this furnace consists in raising the temperature of the fragmentary mass of .ore to 1700'F.', maintaining this temperature .under neutral or slightly reducing combustion conditions for a period of approximately one'hour to permit the heat to penetrate throughout the mass, then shutting off the air supgily pamin natural gas through the charge or a-perio of from four -to six hours. By the end of thistime the mass will have assumed a barely visible red heat and will have dro ped in temperature to' about 900 F. At t e end of the gas or reducing period, as it is called, the gas is shut off and the converter tilted on its trunnions to dump the charge as quickly as possible in order that it may cool within a matter of minutes to reduced particles.

The real reduction of'the ore commences when the airis shut off at the furnace, and

prevent reoxidation of the the reduced ore has a slate gray appearancewith a' beautiful lustre somewhat similar to that of the mineral galena. In fracture it is cubical, quite similar also to gale'na. In the reduction of the-ore it is essential to avo d overheatin the same for a temperature in excess of 1 00 F..tends to produce ferrous silicate and the latteris entirely non-mag netic and would of course prevent certain magnetic separation to be hereafter described.

The reduced ore is .now passed through a jaw crusher and ball mill or set of rolls to imately' to athree partso comminute it to particles ranging from 8 mesh to fines. During the milling operation a strong suction is maintained on the milling apparatus which tendsto draw out all very finely divided particles in which practically .all of the clay-like substance previously referred to is to be found. This air floated powder constitutes a waste product and is thrown away. It comprises ap roximately five percent of the tota weight (518,! (1 into the mill. On passing from the mi theremainder, relieved of its impalpable flour, is passed over a 40 mesh screen t rough which pass the grains rich in free silica or quartz.

As the quartz is undesirable the minus40 product constitutes a. second loss of tailings product for which at present we have no use ut which may in-the future prove of some value. The second tailings roduct c nstitutes approximately 15% of t e total eight of ore charged into the mill.

comprises .about 73% of the original weight of crude ore, which recovery it will be seen, represents a very high one in the light of ordinary 'concentration operations some of which recover but a few percent of the ore charged into the mill. 7

. The resulting, product shows a chemical composition of apgiroximately 52% alumina" 46% of silica an usually less than 2% 0 combined fluxes such as ironoxide, titania,

the magnetic separator it ispossible to eliminate practically all of the remaining impurities but wedo not find it necessary or desirable to do this except where a pure white ceramic material must be made.

It is important to observe the relatively large proportion of alumina to silica thus obtained, and care should be...exerci .in the selection'of minerals for treatment according to the present process that are sufficiently rich in alumina to give the proportions recited amountin almost or approxaluminatotwoparts of silica Theoreticall perfect yro hyllite is indicated by the ormula Al SiO.'),, the constituents bein ica, 28.3 alumina an 5.0 water; but in the selection of the pyrophyllite above referred indicated as 66.7 sil- I magnesia and lime. By reconcentration over 1 lao to, it is obvious that a greater richness of practically all ceramists the world over; andl a r for treatment, whereby the final product comprises approximately 52% of alumina to 46% silica should be selected because of its richness inalumina rather than because of its classification as pyrophylhte'.

The finished product in grain form is next char d into a ball mill or pebble mill or any suita 1e grinding machine which produces a large (percentage'of veryl fine flour andis groun to pass an 80 mes screen. The fine powder thus produced forms the finished product ready for use in the ceramic industry. I

An exhaustive series of tests under practical commercial working conditions shows that this product imparts certain valuable characteristics to burnt clay wares as hereinbefore outlined, a number of which will be enumerated. more specifically and described in detail below.

. Mechanical strength 7 An admixture of 10%of my compound with 90% of English ball clay, made into a briquette, and fired in a ceramic kiln to cone 18 shows a resistance to impact of about 40 to 1 over the fired strength of the English ball clay alone. English ball clay is referred to and used for test purposes, first, because it is a standard ceramic material known to second, because it is one of the strongest bond clays' known to the art. It is significant therefore that an addition of but 10% of my compound to this already strong clay should so greatly enhance its toughness. The addition of to English ball clay increases its fired stren h approximately 140 Englishball clayincreases the strength 158 times. The significance ofthis characteristic will be apparent at once when the relation of strength to durability of my burnt clay articles is takeninto account, such as for instance ordinary crockery and earthenware, stone ware, whiteware, and china, terracotta building material, bricks and other articles made ofbnrnt clay practicall i all of which may be enhanced in strength t rough the addition of small percentages of my compound. It is notable that careful experiments show the above specified percentages to be the critical advantageous 'proportionings of my composition and clay. Increases or decreases in percentages relative to those stated do not appear to afford material advantages as my experiments thus far enlighten me. Nevertheless approximately the stated proportions affor effective results.

The precise action which takes place incident to the use of my product or composition, when combined with ceramic compositions of a clay nature, I cannot describe for at present the knowledge of ceramists of reactions that take place in clay which times while the additidn of to 30% of bodies as they are fired is based largely upon conjecture and is too meager to be much res lied upon. In the combination of my composition with clay, however Ithink'that the accuracy which is now impossible it is believed that burnt clay represents 'amass of microsco ic crystals of unknown composition held together by a cementing matrix of relativel fusible glass; The strength of the burnt c ay shapes is therefore a function i of the strength and toughness of the glass cements its Through the introduction of my improved product I introduce into the composition of the clay a greatly increased percentage of these crysta s of unknown composition with the result that the percentage of crystals may grow to such proportions as'to present an interlocking structure in which the glass merely fills the voids'between the crystals acting rather as a pore filler than as a cement. Thistheory I believe to be substan/ tiated by the fact that increasing percentages of my improved product in a clay body almost invariably result in great increased strength and toughness.

Refractory properties composition has been added will bear a greater load at high temperature than a brick particles together.

made of the same clay without the-addition.

of said composition. Inother words, the rigidity of the mass at high temperature is increased.

Therefore, it becomes apparent that additions of my product to bond clays will improve the refractory qualities of the bond uct added to a plastic fire clay is of exceptional advantage because of itsproperty of eliminating the'fire shrinkage in clay bodies. Admixed with the 8 to 40 mesh concentrate of my composition such a cement forms 'a valuablemixture for ramming or tamping into small. furnaces to make a monolithic lining. The same admixture may be pressed or molded .into bricks fired in an ordinary ceramic kiln in which case the resulting bric will have practically all of the stable prop-. erties of the new product itself.

My final product may be described as a silicate of alumina of peculiar physical structure. A typical analysisshows a ratio of unique. J

. mass quickly to prevent reoxidation, and meassociated therewith contained therein, and

mechanically comminuting the resultinging the mass to chanically comminuting the resulting product.-

' 2. The rocess of making a ceramic material, whic consists of sub]ecting pyrophyllite to reduction by heat, cooling the re uced mass quickly to prevent reoxidation, separating out of the mass undesired materials product. 4 p 3. The process of making a ceramic mate- "ial, which consists of subjecting pyrophyllite to reduction by heat, cooling the reduced mass quickly to prevent reoxidation, crusharticles ranging from 8 mesh to fines, and drawing oil by suction undesired materials associated therewith and contained inthe crushed mass, and mechanically'comminuting the resulting product.

- 4. The rocess of making a ceramic mateial, whic consists'of sub ecting pyrohylvlite to reduction by heat, cooling the re uced mass quickly to prevent reoxidation, crush-- ing the mass to articles ranging from 8 mesh to fines, an drawing off by suction undesired materials associated therewith and contained in the crushed mass, removing from the mass'the free silica, and mechanie cally comminuting the resulting product.

2 5. The process of making a ceramic material, which consists of subjecting'pyrophyllite to reduction by heat, cooling the reduced mass quickly to preventreoxidation,, crushingthe-mass to particles ranging from 8 mesh to fines, and drawing ofi by suction undesired materials. associated therewith and product an contained in the crushed mass, removing from the mass the free silica, subjecting the mass to magnetic separative action to remove other impurities contained therein,"and mechan-.

ically comminuting the resulting product.

6. The process of making a ceramic materialwhich consists of subjecting pyrophyl mass quickly to prevent reoxidation, and mechanicall comminuting the resulting grinding the, residue to a fine powder for use.

71 A composition for ceramic uses consisting of substantially pure residuum obtained from the pyrochemlcal reduction of pyrophyllite.

8. A composition for ceramic uses consisting of the substantially pure concentrated residuum obtained from the pyrochemical reduction of pyrophyllite ore.

9. A composition for ceramic uses consisting of finely comminuted substantially pure -lite to reductionby heat, cooling the reduced concentrated residuum obtained-from the pyrochemical reduction of pyrophyllite ore.

10: A composition for ceramic uses consisting of the substantially pure concentrated residuum obtained from the pyrochemical re duction of pyrophyllite ore, the concentrated residuum having substantially all free metallic oxides removed therefrom.

11. A composition :Eor ceramic use, comprising a mineral product from which substantially all undesirable materials associ- 'ated therewith have been removed, and in which alumina and silica are retained in pro-- portions of'a preponderance of alumina, the product being substantially pure residuum obtained from the'pyrochemical reduction of pyrophyllite.

12. A composition for ceramic use, pomprising a mineral concentrate from which substantially all undesirable materials associated therewith have been removed, and in which alumina and silica are retained in proportions of not less than fifty per cent (50%) alumina, the mineral concentrate being sub--.

stantially pure residuum obtained from the .pyrocheinical reduction of pyrophyllite ore.

13. A composition for ceramic'use, comprising a mineral concentrate from which substantially all undesirable materials associated therewith have been removed and in which alumina and silica are retained in proportions of approximately three of the former the sillimanite class and conditioned to mixed with ceramic clay for counteracting shrinkage therein, the said mineral concentrate bemg substantially pure concentrated residuum obtained from the pyrochemical eduction of pyrophyllite ore.

In testimony whereof I aflix in si ature. THOMAS S. A TIS. 

